Isotope effect in formaldehyde steam reforming on Pt/m-ZrO2: Insight into chemical promotion by alkalis

Michela Martinelli; Jonas Marcelle; Donald C. Cronauer; A. Jeremy Kropf; Gary Jacobs

doi:10.1016/j.catcom.2023.106668

Isotope effect in formaldehyde steam reforming on Pt/m-ZrO₂: Insight into chemical promotion by alkalis

Michela Martinelli
, Jonas Marcelle
, Donald C. Cronauer
, A. Jeremy Kropf
, Gary Jacobs

Producción científica: Article › revisión exhaustiva

2 Citas (Scopus)

Resumen

Infrared spectroscopy, temperature programmed reaction mass spectrometry (TP-reaction/MS), and catalyst testing were used to investigate alkali promotion of dehydrogenation selectivity during formaldehyde steam reforming (FSR) on Pt/m-ZrO₂. In a preferred pathway, formaldehyde reacts with water forming hydrogen and formate, followed by forward formate decomposition to CO₂ and H₂. Alkali-doping of 2 wt% Pt/m-ZrO₂ increases catalyst basicity, which weakens the formate C–H bond promoting formate dehydrogenation / decarboxylation. Promotion by alkali in FSR was observed through a formate ν(CH) band shift to lower wavenumbers in infrared spectroscopy, and through a decrease in the normal isotope effect in switching from H- to D-labeled formaldehyde in TP-reaction/MS.

Idioma original	English
Número de artículo	106668
Publicación	Catalysis Communications
Volumen	178
DOI	https://doi.org/10.1016/j.catcom.2023.106668
Estado	Published - may 2023

Nota bibliográfica

Publisher Copyright:
© 2023 The Authors

Financiación

The work of Gary Jacobs and Jonas Marcelle was funded in part by a UTSA-SWRI Connect grant supported by The Office of the Vice President for Research, Economic Development, and Knowledge Enterprise at UTSA . Argonne's research was supported in part by the U.S. Department of Energy (DOE) , Office of Fossil Energy , National Energy Technology Laboratory (NETL) . The Advanced Photon Source was supported by the U.S. Department of Energy , Office of Science , Office of Basic Energy Sciences , under contract number DEAC02-06CH11357 . MRCAT operations are supported by the Department of Energy and the MRCAT member institutions. CAER research was supported by the Commonwealth of Kentucky.

Financiadores	Número del financiador
Office of the Vice President for Research
UTSA-SWRI
U.S. Department of Energy
Office of Fossil Energy and Carbon Management
Office of Science Programs
DOE Basic Energy Sciences	DEAC02-06CH11357
National Energy Technology Laboratory

ODS de las Naciones Unidas

Este resultado contribuye a los siguientes Objetivos de Desarrollo Sostenible

Affordable and clean energy

ASJC Scopus subject areas

Catalysis
General Chemistry
Process Chemistry and Technology

Acceder al documento

10.1016/j.catcom.2023.106668

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title = "Isotope effect in formaldehyde steam reforming on Pt/m-ZrO2: Insight into chemical promotion by alkalis",

abstract = "Infrared spectroscopy, temperature programmed reaction mass spectrometry (TP-reaction/MS), and catalyst testing were used to investigate alkali promotion of dehydrogenation selectivity during formaldehyde steam reforming (FSR) on Pt/m-ZrO2. In a preferred pathway, formaldehyde reacts with water forming hydrogen and formate, followed by forward formate decomposition to CO2 and H2. Alkali-doping of 2 wt\% Pt/m-ZrO2 increases catalyst basicity, which weakens the formate C–H bond promoting formate dehydrogenation / decarboxylation. Promotion by alkali in FSR was observed through a formate ν(CH) band shift to lower wavenumbers in infrared spectroscopy, and through a decrease in the normal isotope effect in switching from H- to D-labeled formaldehyde in TP-reaction/MS.",

keywords = "Alkali, Formaldehyde steam reforming, Hydrogen production, Isotope effect, Platinum / zirconia, Sodium",

author = "Michela Martinelli and Jonas Marcelle and Cronauer, \{Donald C.\} and Kropf, \{A. Jeremy\} and Gary Jacobs",

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T2 - Insight into chemical promotion by alkalis

AU - Martinelli, Michela

AU - Marcelle, Jonas

AU - Cronauer, Donald C.

AU - Kropf, A. Jeremy

AU - Jacobs, Gary

PY - 2023/5

Y1 - 2023/5

N2 - Infrared spectroscopy, temperature programmed reaction mass spectrometry (TP-reaction/MS), and catalyst testing were used to investigate alkali promotion of dehydrogenation selectivity during formaldehyde steam reforming (FSR) on Pt/m-ZrO2. In a preferred pathway, formaldehyde reacts with water forming hydrogen and formate, followed by forward formate decomposition to CO2 and H2. Alkali-doping of 2 wt% Pt/m-ZrO2 increases catalyst basicity, which weakens the formate C–H bond promoting formate dehydrogenation / decarboxylation. Promotion by alkali in FSR was observed through a formate ν(CH) band shift to lower wavenumbers in infrared spectroscopy, and through a decrease in the normal isotope effect in switching from H- to D-labeled formaldehyde in TP-reaction/MS.

AB - Infrared spectroscopy, temperature programmed reaction mass spectrometry (TP-reaction/MS), and catalyst testing were used to investigate alkali promotion of dehydrogenation selectivity during formaldehyde steam reforming (FSR) on Pt/m-ZrO2. In a preferred pathway, formaldehyde reacts with water forming hydrogen and formate, followed by forward formate decomposition to CO2 and H2. Alkali-doping of 2 wt% Pt/m-ZrO2 increases catalyst basicity, which weakens the formate C–H bond promoting formate dehydrogenation / decarboxylation. Promotion by alkali in FSR was observed through a formate ν(CH) band shift to lower wavenumbers in infrared spectroscopy, and through a decrease in the normal isotope effect in switching from H- to D-labeled formaldehyde in TP-reaction/MS.

KW - Alkali

KW - Formaldehyde steam reforming

KW - Hydrogen production

KW - Isotope effect

KW - Platinum / zirconia

KW - Sodium

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